CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Xuan Huang,Ming Yi,Kewen Tang
To address resources shortage and environmental degradation, noble metal recovery from e-waste is in desperate need. Herein, to achieve selective extraction of gold (Au) and palladium (Pd) from practical e-waste, a series of tridentate thioether extractants are designed with ester functional groups at both ends of the thioether. By varying the chain length of the ester alkyl, the relationship between extractant structure and performance is further explored. The results indicate that the as-introduced tridentate structure facilitate the Au(III) and Pd(II) extraction, demonstrating a complex mechanism involving both coordination substitution and ion association. Notably, the extractant with the shortest carbon chain length and smallest molecular weight delivers outstanding extraction capacities of 920.2 mg/g for Au(III) and 280.7 mg/g for Pd(II). More importantly, it exhibits superior selectivity (∼100 %) for Au(III) and Pd(II) in complex metal solutions. This work guides the design of thioether-based extractants for sustainable recovery of noble metal from practical e-waste.
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Journal of Environmental Sciences
·
2021
·
IF 5.565
Chang Cui,Yan Zhang,Wenpo Shan,Yunbo Yu,Hong He
Alumina supported Pd catalyst (Pd/Al 2 O 3 ) is active for complete oxidation of methane, while often suffers transient deactivation during the cold down process. Herein, heating and cooling cycle tests between 200 and 900°C and isothermal experiments at 650°C were conducted to investigate the influence of NO x on transient deactivation of Pd/θ-Al 2 O 3 catalyst during the methane oxidation. It was found that the co-fed of NO alleviated transient deactivation in the cooling ramp from 800 to 500°C, which was resulted from the in situ formation of NO 2 during the process of methane oxidation. Over the Pd/θ-Al 2 O 3 , thermogravimetric analysis and O 2 temperature programmed oxidation measurements confirmed that transient deactivation was due to the decomposition of PdO particles and the hysteresis of Pd reoxidation, while the metal Pd entities were less active for methane oxidation than the PdO ones. CO pulse chemisorption and scanning transmission electron microscopy characterizations rule out the NO 2 effect on Pd size change. Powder X-ray diffraction and X-ray photoelectron spectroscopy characterizations were used to obtain palladium status of Pd/θ-Al 2 O 3 before and after reactions, indicating that in lean conditions at 650°C, the presence of NO 2 increases the content of active PdO on the catalyst surface, thus benefits methane oxidation. Homogeneous reaction between CH 4 , O 2 , and NO x may be partially responsible for the alleviation above 650°C. The interesting research of alleviation in transient deactivation by NO x , the components co-existing in exhausts, are of great significance for the application.
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Reaction Kinetics Mechanisms and Catalysis
·
2022
·Vol. 135
·期 6
·3243-3256
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IF 1.843
Zhou Lin,Wang Ruo-Bing
Nitrogen doped mesoporous carbon (N-MPC)-supported monometallic and bimetallic catalysts were synthesized by using hydrothermal and impregnation method, and the catalytic activity of the catalyst to carbon–carbon bond-forming reactions (Suzuki, Heck and Sonogashira reactions) was studied. The bimetallic catalyst Pd-Ni@N-MPC with high Ni to Pd atomic ratios showed highly activity in the C–C coupling reactions of aryl halide under optimized condition. In contrast to their monometallic counterparts, such Pd-Ni@N-MPC catalyst not only show higher catalytic activity but also show more economic and stable. The catalysts were characterized by powder X-ray diffraction, X-ray photoelectron spectroscopy, scanning electron microscope and transmission electron microscopy, which demonstrated that the Pd–Ni NPs highly dispersed and possessed uniform size.
Graphical abstract
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JOURNAL OF CATALYSIS
·
2021
·
IF 7.92
Zhi-Feng Jiao,Ya-Ming Tian,Xiao-Ning Guo,Udo Radius,Holger Braunschweig,Todd B. Marder,Xiang-Yun Guo
A highly efficient photocatalytic protocol for borylation of alkyl bromides and chlorides with graphene supported Cu/Pd alloy nanoparticles as a heterogeneous catalyst is reported. This photocatalytic system operates with visible light in air, providing a wide range of primary and secondary alkyl halides with B 2 pin 2 or B 2 neop 2 in high yields at low temperatures, thereby demonstrating its broad utility and functional group tolerance. The high performance is attributed to a synergistic effect of localized surface plasmon resonance (LSPR) of Cu and charge transfer from Cu to Pd due to the alloy surface charge heterogeneity. Transfer of energetic electrons from Pd to electrophilic alkyl halides lead to the formation of the alkyl radicals, which quickly react with a nucleophilic adduct of a diboron compound with base adsorbed on the positively charged Cu sites to form the corresponding borylation product.
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AICHE JOURNAL
·
2025
·Vol. 71
·期 8
·e18862
·
IF 4
Yue Zhang,Rongrong Zhang,Shuzhen Lyu,Xiangwei Ren,Guozhu Liu,Li Wang
Supported Pd-based nanoparticles are widely regarded as the most effective catalysts for 2-ethylthraquinone hydrogenation. Herein, the heteroenergetic dual-supports were prepared by coating resorcinol-formaldehyde (RF) resin on mesoporous SBA-15 to regulate the growth and surface microenvironment of Pd. After calcination and reduction, phenolic hydroxyl groups in the residual carbon layer effectively reduced the Pd particle size, induced the formation of adjacent Pd 0 –Pd δ+ , and created hydrophobicity. Density functional theory calculations revealed that Pd atoms preferentially interact with OH on C, rather than with OH on SBA-15, providing an intrinsic driving force for smaller Pd particle size. The mass ratio of RF to SBA-15 was shown to be a crucial parameter affecting the catalytic performance. At the ratio of 4 (carbon content of 2.02%) the catalyst possesses the smallest Pd particles, 30% Pd δ+ proportion, and higher hydrophobicity, achieving the best catalytic performance, with an activity of 0.57 molH 2 ·gPd −1 ·min −1 and a selectivity of 95.3%.
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Acta Pharmaceutica Sinica B
·
2025
·
IF 14.6
Yuhong Wang,Lin Hu,Lei Wang,Chonghai Zhang,Wenhao Shen,Hongli Yang,Min Li,Xin Zhang,Mengmeng Xu,Muxing Zhang,Kai Yang,Xiaopeng Tian
Inflammatory bowel disease (IBD) is an autoimmune disorder involving complex immune regulation, where balancing localized and systemic immunosuppression is a key challenge. This study aimed to enhance the therapeutic efficacy by engineering the probiotic Escherichia coli Nissle 1917 (EcN). We removed endogenous plasmids pMUT1 and pMUT2 from wild-type EcN and expressed the mPD-L1 (19‒238 aa)-mFc fusion protein on the bacterial surface using a cytolysin A (ClyA) fragment. This modification stabilized mPD-L1 (19‒238 aa) protein expression and promoted its recruitment to outer membrane vesicles (OMVs). The engineered strain, EcNΔ pMUT1/2 -ClyA-mPD-L1-mFc (EcN-ePD-L1-mFc), features conditional ePD-L1-mFc expression under the araBAD promoter, enhancing gut-targeted release and reducing systemic side effects. This strain improved treatment targeting and efficiency by enabling direct ePD-L1-mFc interaction with immune cells at inflammation sites. OMVs from this strain induced Treg proliferation, inhibited effector T cell proliferation in vitro , and significantly improved intestinal inflammation and colonic epithelial barrier repair in vivo . Additionally, the bacterium restored intestinal microbiota balance, increasing Lactobacillaceae and reducing Bacteroides . This study highlights the engineered bacterium's potential for targeted intestinal immune modulation and offers a novel local IBD treatment approach with promising clinical prospects.
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JOURNAL OF ORGANIC CHEMISTRY
·
2025
·
IF 3.6
Jiapeng Sun,Hanxiao Luo,Junyong Wang,Hongliang Li,Raorao Zheng,Dingru Qiao,Jiaji Zhao,Yue Yu,Hua Cao
A simple and practical method has been developed for the carbonylative esterification of imidazo[1,2-a]pyridines via C(sp2)–H bond functionalization using alkyl alcohols under mild reaction conditions. The carbonyl fragment is sourced from radical-mediated C–C cleavage of the alcohols, providing a green, safe, and economic alternative to traditional carbonyl sources like carbon monoxide. Through this strategy, a number of imidazo[1,2-a]pyridine-3-carboxylates were obtained from simple substrates by a single step.
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ACS Applied Nano Materials
·
2024
·
IF 5.3
Binghui Zhou,Xinlei Ding,Yun Chen,Hanyang Wang,Yadong Liu,Chengfei Wang,Guangmei Bai,Wenge Qiu
The activation process is a key step in preparing porous carbon. Herein, three kinds of green activators were separately used to successfully prepare N-doped porous carbons through a two-step strategy: hydrothermal carbonization and chemical activation using microcrystalline cellulose as the carbon source and urea as the nitrogen source. Palladium was deposited on these N-doped microcrystalline cellulose-based carbons (NMC-X, where X represents the activator) via a traditional deposition–precipitation method, and the resulting Pd nanoparticle catalysts (Pd/NMC-X) showed high activity in the selective hydrogenation of quinoline under mild conditions, particularly Pd/NMC-ZC (ZC, zinc carbonate), which achieved complete conversion of quinoline within 100 min at 40 °C and 4 atm H2. Characterization results suggest that the high activity of Pd/NMC-ZC is mainly attributed to the special electronic structure of its Pd species, particularly the distribution of valence states and reducibility of Pd and the high hydrogen spillover capacity between Pd and NMC-ZC. The chemical activation by ZC leads to the formation of multiple defect sites on the carbon skeleton, modifying the carbon surface properties to enhance hydrogen spillover. This also provides an excellent environment for Pd nanoparticle anchoring, thus increasing the Pd-support interactions and regulating the electronic structure of Pd.
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DALTON TRANSACTIONS
·
2025
·
IF 3.3
Yonghui Ye,Yu Zhang,Xintong Yan,Gong Ning,Shi Hu
A facile one-step method is employed to synthesize carbon-supported Pd–Pb binary metal catalysts for the ethanol oxidation reaction (EOR) in alkaline electrolytes. A variety of characterization techniques have demonstrated that the alloying of Pd with Pb alters the electronic structure and induces lattice expansion. Electrochemical tests for the EOR in alkaline electrolytes demonstrated that the Pd3Pb/C catalyst exhibited the highest mass activity (3.59 A mgPd−1) and specific activity (17.97 mA cm−2), which are 4.6 and 4.7 times those of the Pd/C catalyst prepared by the same method, respectively. The intercalation of lead atoms has altered both the lattice and the electronic structure of palladium, leading to opposing shifts in the d-band center that collectively optimize the adsorption strength of CO* and OH*, key intermediates of the EOR. Consequently, the Pd3Pb/C electrocatalyst exhibits significant EOR catalytic activity. This study provides a viable implementation plan and analytical strategy for optimizing palladium-based catalysts with non-noble metals by integrating electronic transfer, bifunctional effects, and d-band center adjustments for bimetallic catalysts.
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Frontiers in Immunology
·
2025
·
IF 5.9
Dong-Ni Pei,Yang Song,Ying-Xia Zhou,Bo Shu,Shao-wei Huang,Fa-Zhao Li,Wei-Dong Dai,Bao-Ye Sun
Purpose Conventional type 1 dendritic cells (cDC1s) mastermind anti-cancer immunity and play a pivotal role in determining the efficacy of cancer immunotherapies. In this study, we sought to decipher the dynamic changes in the tumor immune landscape during intrahepatic cholangiocarcinoma (iCCA) development and harness the therapeutic potential of targeting cDC1s for cancer therapy. Methods We constructed spontaneous murine iCCAs via hydrodynamic tail vein injection (HDTVi) of plasmids encoding AKT/YAP. To characterize tumor-infiltrating immune cell populations throughout iCCA carcinogenesis and progression, we performed time-of-flight mass cytometry (CyTOF). To expand and activate cDC1s, we combined Flt3L with poly I:C (FL-pIC) therapy and assessed its therapeutic efficacy in both AKT/YAP-induced iCCAs and a subcutaneous tumor injection model. Flow cytometric analyses were used to evaluate intra-tumoral infiltration levels of cDCs and CD8 + T cells. Results CyTOF analysis revealed the progressive formation of an immunosuppressive tumor microenvironment as iCCA advances. Crucially, infiltration of cDC1s dramatically decreases in advanced iCCAs compared to early-stage tumors. Combined FL-pIC therapy preferentially expanded CD103 + cDC1s, powerfully inhibiting tumorigenesis in AKT/YAP-driven murine iCCAs and sensitizing these tumors to anti-PD-1 therapy. Moreover, FL-pIC therapy markedly suppressed the growth of established mIC-23 subcutaneous tumors. Conclusions Our findings demonstrate that recruiting and activating intra-tumoral cDC1s is feasible and essential for driving anti-tumor CD8 + T cell immune responses and enhancing anti-PD-1 therapeutic effectiveness in iCCA.
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GREEN CHEMISTRY
·
2025
·
IF 9.2
Jianfeng Lin,Xuri Wu,Yijun Chen
Statins, leading cholesterol-lowering drugs, contain a pivotal pharmacophore side chain. However, the Pd/C-catalyzed debenzylation step in the side chain production poses a series of cost and environmental issues. In this study, an efficient debenzylase is generated from the engineering of CYP102A1 to replace the tedious and harmful chemical debenzylation. The engineering process for the debenzylase is primarily enabled by continuous dynamic protein conformational alteration-guided mutagenesis, a newly developed protein dynamics-based strategy to facilitate the prediction of the key residues of both proximal and challenging distal sites, for the improvement of activity and selectivity. Through iterative combinatorial mutagenesis, the best mutant exhibits a 22.6-fold improvement in the total turnover number and an increase in the debenzylating selectivity from 12.2% to 99.8%. Furthermore, the practical value of the debenzylase is demonstrated by incorporating a diketoreductase-mediated synthetic route through an enzymatic cascade reaction to produce an advanced precursor of statins. This study not only establishes the first enzymatic alternative to the removal of the widely used benzyl group in organic synthesis but also paves the way for accelerating enzyme engineering in a rational manner.
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Advanced Science
·
2025
·
IF 14.1
Sisi Yao,Jiawei Han,Wenjun Zhang,Dengkang Guo,Shenjie Han,Yun Lu,Jingpeng Li
Developing efficient catalytic hydrogenation microreactors with minimal catalyst loading yet high active-site density for treating concentrated organic pollutants remains challenging. Herein, a facile room-temperature method is presented to stabilize Pd single-atom catalysts (SACs) within ZIF-67 crystals during their formation, aiming to fabricate an efficient, low-loading hydrogenation catalytic microreactor (Pd@Z-P/b CMR). ZIF-67 is constructed into polydopamine (PDA)-modified bamboo microchannels under flow conditions, utilizing preimmobilized Co 2+ seeds in PDA. Despite an ultralow Pd loading (0.0014 wt.%), the Pd@Z-P/b CMR featuring atomically dispersed Pd─N 4 sites in ZIF-67 considerably outperforms its Pd nanoparticle–loaded counterpart (Pd 0.0035 wt.%) in continuous-flow hydrogenation, demonstrating superior robustness and maximized Pd utilization with 94.3% conversion efficiency for saturated 4-nitroaniline over 10 d and 97.5% conversion efficiency for gram-level methylene blue (1.0 g L −1 ) over 5 d. Crucially, it exhibits consistent, high performance in real environmental water samples. The high surface area and porosity of ZIF-67 stabilize the Pd SACs, enhance dispersion, and ensure accessibility. Simultaneously, the Pd─N 4 configuration facilitates electron transfer and optimizes hydrogen binding energy, dramatically boosting the catalytic activity. This work provides a novel strategy for room-temperature SAC synthesis and the effective treatment of high-concentration organic pollutants for sustainable wastewater remediation.
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